EP0242776A1 - Gas-Flüssigreaktor und Verfahren zum Mischen von Gas mit Flüssigkeit - Google Patents

Gas-Flüssigreaktor und Verfahren zum Mischen von Gas mit Flüssigkeit Download PDF

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Publication number
EP0242776A1
EP0242776A1 EP87105515A EP87105515A EP0242776A1 EP 0242776 A1 EP0242776 A1 EP 0242776A1 EP 87105515 A EP87105515 A EP 87105515A EP 87105515 A EP87105515 A EP 87105515A EP 0242776 A1 EP0242776 A1 EP 0242776A1
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EP
European Patent Office
Prior art keywords
liquid
gas
vessel
reactor
head space
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP87105515A
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English (en)
French (fr)
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EP0242776B1 (de
Inventor
Joseph J. Concordia
Donald R. Hall
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Herzog-Hart Corp
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Herzog-Hart Corp
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Publication date
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Publication of EP0242776A1 publication Critical patent/EP0242776A1/de
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Publication of EP0242776B1 publication Critical patent/EP0242776B1/de
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Expired - Lifetime legal-status Critical Current

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J4/00—Feed or outlet devices; Feed or outlet control devices
    • B01J4/001—Feed or outlet devices as such, e.g. feeding tubes
    • B01J4/002—Nozzle-type elements
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
    • B01F25/20—Jet mixers, i.e. mixers using high-speed fluid streams
    • B01F25/21—Jet mixers, i.e. mixers using high-speed fluid streams with submerged injectors, e.g. nozzles, for injecting high-pressure jets into a large volume or into mixing chambers
    • B01F25/211—Jet mixers, i.e. mixers using high-speed fluid streams with submerged injectors, e.g. nozzles, for injecting high-pressure jets into a large volume or into mixing chambers the injectors being surrounded by guiding tubes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/232—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids using flow-mixing means for introducing the gases, e.g. baffles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/234—Surface aerating
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/234—Surface aerating
    • B01F23/2341—Surface aerating by cascading, spraying or projecting a liquid into a gaseous atmosphere
    • B01F23/23413—Surface aerating by cascading, spraying or projecting a liquid into a gaseous atmosphere using nozzles for projecting the liquid into the gas atmosphere
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/2366—Parts; Accessories
    • B01F23/2368—Mixing receptacles, e.g. tanks, vessels or reactors, being completely closed, e.g. hermetically closed
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/40—Mixing liquids with liquids; Emulsifying
    • B01F23/45—Mixing liquids with liquids; Emulsifying using flow mixing
    • B01F23/454—Mixing liquids with liquids; Emulsifying using flow mixing by injecting a mixture of liquid and gas
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/2455—Stationary reactors without moving elements inside provoking a loop type movement of the reactants
    • B01J19/246—Stationary reactors without moving elements inside provoking a loop type movement of the reactants internally, i.e. the mixture circulating inside the vessel such that the upward stream is separated physically from the downward stream(s)
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
    • B01F25/50—Circulation mixers, e.g. wherein at least part of the mixture is discharged from and reintroduced into a receptacle
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S261/00—Gas and liquid contact apparatus
    • Y10S261/75—Flowing liquid aspirates gas

Definitions

  • This invention relates to a reactor for transferring a reactive gas to a liquid and, more particularly, to a gas-liquid reactor having a high rate of gas transfer into the liquid and to a method for effectively transferring a reactive gas to a liquid.
  • Apparatus for gas-liquid mixing is used for many chemical reaction processes and fermentation processes.
  • a liquid to be reacted is placed in a reactor vessel.
  • the liquid contains compounds to be reacted or cells which take part in a fermentation process.
  • a gas is introduced into the liquid by a variety of techniques, and a reactive component of the gas reacts with the liquid in a desired manner.
  • a variety of techniques has been used for gas-liquid mixing including mechanically agitated tanks, sparged gas columns and nozzle assemblies to disperse gas in a liquid.
  • One widely used gas-liquid reactor includes a submerged jet nozzle at the bottom of a cylindrical vessel, and a guide tube coaxial with the cylindrical vessel and positioned over the submerged jet nozzle.
  • a gas-liquid mixture injected by the nozzle, circulates upwardly through the guide tube to the surface of the liquid and then downwardly in the annular space outside the guide tube, resulting in continuous circulation.
  • a so-called free jet nozzle is positioned at the top of a vessel in the head space above the liquid surface. Reactive gas is introduced into the head space and is entrained by the downwardly injected liquid jet from the free jet nozzle.
  • a gas-liquid reactor comprising a vessel for containing a liquid, the vessel having a sidewall, a top and a bottom, a submerged jet nozzle positioned at the bottom of the vessel for injecting a liquid and gas mixture upwardly into the liquid in the vessel and at least two free jet nozzles positioned at the top of the vessel in a head space above the liquid surface for injecting a liquid jet downwardly into the liquid in the vessel.
  • Reactive gas in the head space is entrained into the liquid jet and mixed into the liquid in the vessel.
  • the gas-liquid reactor further includes means for supplying reactive gas to the submerged jet nozzle, means for supplying liquid to the submerged jet nozzle and to the free jet nozzle, means for venting reacted gas from the vessel, and baffle means for directing reactive gas from the liquid to the head space for entrainment in the liquid jet from the free jet nozzle and for directing reacted gas to the venting means.
  • the vessel preferably comprises an upright cylinder closed at both ends and a cylindrical guide tube coaxial with the vessel.
  • the submerged jet nozzle is positioned on the axis of the vessel and directs a gas-liquid mixture upwardly through the guide tube. The gas-liquid mixture then circulates downwardly through the annular region between the guide tube and the vessel wall.
  • the gas liquid reactor of the present invention is preferably provided with diffuser tubes extending from each free jet nozzle downwardly into the liquid in the vessel in the annular space between the guide tube and the vessel wall.
  • the diffuser tubes cause the gas-liquid mixture generated by the free jet nozzle to be injected into the lower portion of the vessel.
  • the diffuser tubes increase in diameter toward the bottom of the vessel to facilitate transfer of the gas-liquid mixture into the lower portion of the vessel.
  • the baffle means preferably includes a first horizontal baffle plate positioned in the head space above the liquid and a cylindrical baffle member extending downwardly from the first baffle plate into the liquid outside the guide tube. Gas rising from the liquid surface above the guide tube is directed into the head space for recirculation via the free jet nozzles while gas rising from the liquid in the annular space outside the guide tube is directed to the venting means.
  • a method for mixing a gas into a liquid in a gas-liquid reactor vessel comprises the steps of injecting liquid and gas upwardly into the liquid in the vessel from a submerged jet nozzle positioned at the bottom of the vessel, injecting liquid and gas, which is entrained into the liquid from the head space in the vessel, downwardly into the liquid in the vessel from at least two free jet nozzles positioned in the head space, and directing reactive gas from the liquid to the head space for entrainment in the liquid jet from the free jet nozzle while directing reacted gas from the liquid to a vent.
  • a gas-liquid reactor in accordance with the present invention is illustrated in FIGS. l, lA and 2.
  • a vessel l0 includes a cylindrical sidewall l2, a top l4 and a bottom l6.
  • the vessel l0 may be fabricated from any weldable metal such as plain or stainless steel and is positioned with the axis l8 of the cylindrical sidewall l2 oriented vertically.
  • a liquid 20 to be reacted fills the major portion of the vessel l0.
  • Above a liquid surface 22, the top l4 and the sidewall l2 define a head space 24 filled with a gas as described hereinafter.
  • a submerged jet nozzle 30 is mounted in the bottom l6 of the vessel l0 on the axis l8.
  • the nozzle 30 includes an inner nozzle portion 32 which receives pressurized liquid through a conduit 34, and an outer nozzle portion 36 concentric with the inner nozzle portion 32 which receives a reactive gas through a conduit 38 from a gas supply 40.
  • the inner and outer nozzle portions 32, 36 extend through the vessel bottom l6 and terminate within the liquid in vessel l0 in a nozzle tip 42.
  • Liquid is pumped from the inner nozzle portion 32 upwardly into the liquid in the vessel l0. Since the liquid entering the vessel l0 through the jet nozzle 30 has considerable velocity relative to the liquid in the vessel l0, there is created an interface 44 between the relatively fast-moving liquid from the nozzle 30 and the relatively slow-moving liquid in the vessel l0.
  • the interface 44 is generally conical in shape, with the apex of the cone approximately coincident with the nozzle tip 42.
  • the differential liquid velocities at the interface 44 create a shear force which, as noted hereinabove, is beneficial to transfer of gas to the liquid.
  • the gas is introduced through the outer nozzle portion 36 to the tip 42 in a ring concentric with the inner nozzle portion 32, and is directed into the interface 44 to promote entrainment into the liquid.
  • a cylindrical guide tube 46 is positioned within the vessel l0 with its axis coincident with the axis l8.
  • the guide tube 46 terminates below the liquid surface 22 and promotes circulation of the liquid gas mixture in the vessel l0 in a well-defined manner.
  • the gas-liquid mixture injected by the submerged jet nozzle 30 passes upwardly through the guide tube 46, then radially outward near the liquid surface 22 and downwardly through the annular region between the guide tube 46 and the sidewall l2, as indicated by the arrows in FIG. l.
  • the ratio between the diameter of the guide tube 46 and the diameter of the vessel l0 is in the range between 0.5 and 0.6.
  • the guide tube 46 is provided with a heat transfer surface 48.
  • a heat transfer liquid can be circulated from an external source through the passage between surface 48 and the guide tube 46 for heating or cooling of the liquid in vessel l0.
  • the heat transfer surfaces can also be incorporated as part of the diffuser tubes, the vessel wall, or the external liquid recirculation pipes which transfer liquid from the vessel to the nozzles.
  • the free jet nozzles 50, 52 include tubular portions 50a, 52a, which extend from outside the vessel l0 through the vessel top l4 into the head space 24 and terminate in tips 50b, 52b above the liquid surface 22. Liquid is received by the free jet nozzle 50 through a conduit 54 and is injected through the tip 50b downwardly into the liquid in the vessel l0. Similarly, liquid is received by the free jet nozzle 52 through a conduit 56 and is delivered through the tip 52b downwardly into the liquid in the vessel l0.
  • the liquid injected under pressure from the jet nozzles 50, 52 forms liquid jets 60, 62 extending from the nozzle tips 50b, 52b, respectively, downwardly into the liquid in the vessel l0.
  • the liquid jets 60, 62 are generally conical in shape and have turbulence and instability at their surfaces where the liquid interfaces with the gas in the head space 24. The turbulence creates shear force which causes gas in the head space 24 to be entrained into the liquid jets 60, 62 and carried downwardly into the liquid in the vessel l0.
  • the gas-liquid reactor in accordance with the present invention is further provided with diffusers 66, 68 for directing the liquid jets 60, 62, with gas entrained therein, to the lower portion of the vessel l0 for improved gas-liquid mixing.
  • the diffusers 66, 68 are axially oriented with the nozzles 50, 52 and extend from flared ends 66a, 68a adjacent nozzle tips 50b, 52b downwardly into the liquid to outlet apertures 66b, 68b.
  • Upper portions 66c, 68c of the diffusers are uniform diameter tubes while lower portions 66d, 68d are tapered to increase in diameter toward outlet apertures 66b, 68b.
  • the flared ends 66a, 68a form a conical space for directing gas flow toward the liquid jets 60, 62.
  • a low pressure region is created in upper portions 66c, 68c to promote entrainment of gas into the liquid jets 60, 62.
  • the jets attach to the walls and a strong shear plane develops which disperses the gas into small bubbles in the liquid.
  • the tapered lower portions 66d, 68d decrease the velocity and increase the pressure of the gas-liquid mixture flowing downwardly, so that it can be discharged against the pressure existing in the lower portion of the vessel l0.
  • Lower ends of the diffusers 66, 68 are covered by baffles 66e, 68e which direct the gas-liquid mixture outwardly through outlet apertures 66b, 68b.
  • free jet nozzles 50, 52 While two free jet nozzles 50, 52 are included in the present example, it will be understood that additional free jet nozzles can be utilized. In each case, the free jet nozzles are equiangularly positioned about the vessel axis l8 at a radius greater than the radius of the guide tube 46. Also, while the present example describes a particular baffle 66e, 68e at the ends of the diffusers, it will be understood that the termination of the diffuser may have various configurations including, but not limited to, elbows as well as impingement baffles.
  • the gas-liquid reactor of the present invention is provided with a baffle system for separating reactive gases from reacted and substantially inert gases.
  • the baffle system includes a horizontal baffle plate 70 across the vessel l0 above the liquid surface 22.
  • a cylindrical baffle member 72 extends downwardly from the baffle plate 70 into the liquid outside the guide tube 46.
  • the cylindrical baffle member 72 must provide sufficient clearance for liquid recirculation downwardly outside the guide tube 46.
  • An optional third baffle plate 74 is positioned between the baffle plate 70 and the liquid surface 22 above the guide tube 46 and has a diameter slightly larger than the guide tube 46.
  • the horizontal baffle plate 70 is provided with an aperture 76 within the periphery of the cylindrical baffle member 72 and a short pipe 78 extending upwardly from the aperture 76 into the head space 24.
  • the pipe 78 acts as a guide for gas passing upwardly into the head space 24.
  • Gas which circulates upwardly through the guide tube 46 and is partially reacted with the liquid therein, preferably recirculates through the annular region outside the guide tube 46. However, a fraction of the gas rises from liquid surface 22 and passes around the edge of the third baffle plate 74 and upwardly through the aperture 76 into the head space 24. The partially reacted gas is then entrained into the liquid jets 60, 62 as described above and is recirculated into the liquid through diffuser outlet apertures 66b, 68b for more efficient utilization of the reactive gas and a high gas transfer rate. A portion of the gas then passes upwardly through the annular region outside the baffle member 72, as indicated in FIG.
  • baffle configuration 70, 72, 74, 78 to direct gas to the head space 24
  • other means for providing this flow path are available.
  • Another means would be provided by a pipe connection.
  • the gas can be directed through various treatments, including among others, heat exchange, absorption of a gaseous component, drying, or gas enrichment.
  • An external pumping system includes a liquid pump 86, having its outlet coupled via the conduit 34 to the submerged jet nozzle 30, and via conduits 54, 56 to free jet nozzles 50, 52, respectively.
  • a drain 88 from the vessel l0 is coupled via a conduit 90 to the inlet of the pump 86.
  • the external pumping system can be fitted with various other components (not shown) to further process the liquid; for example, a heat exchanger to adjust the liquid temperature, filters to collect solids which may be in the liquid, or special devices to remove and collect valuable products from the liquid.
  • the vessel l0 is filled with liquid to its prescribed capacity prior to operation of the above-described gas mixing system.
  • the vessel is filled to about 35 percent of capacity. Then liquid is gradually added to the system from an external source through the submerged jet nozzles and the free jet nozzles so that gas mixing occurs as the vessel is filled.
  • the reactor of the present example is selected to have a volume of l00 liters and to be used for transfer of oxygen to the liquid.
  • V vessel volume
  • D diameter of the cylindrical vessel
  • H vessel height.
  • V D the volume of the guide tube, is calculated at 28,925 cm3 and V A , the annular volume outside the guide tube, is calculated at 7l,075 cm3 using conventional geometric formulas.
  • the total recirculation per hour, R is selected to be 80 times the vessel volume V or 8,000 liters per hour.
  • the recirculation number n u represents the ratio of the volume of liquid flowing in a loop around the guide tube 46 to the volume of liquid injected into the vessel l0 through the nozzle 30.
  • the recirculation number is in the range between 4 and 6.
  • n u is selected to be 5.
  • the nozzle sizes are selected to give the desired flow rate and to provide a Reynolds number of at least 20,000. Using conventional techniques for calculation of nozzle flow rates and pressure drops, preferred nozzle diameters of 0.2 inches to 0.3 inches are selected.
  • Equation (l0) gives a flow rate, q, of 8.8 cubic feet per minute.
  • the oxygen transfer rates can be estimated. From the above calculations, 8.8 CFM air will be injected through nozzle 30 and 3.28 CFM of air can be injected by means of nozzles 50, 52. It can be determined that the vent gas will be 0.542 pounds per minute of nitrogen gas and 0-0.l65 pounds per minute of oxygen depending on the amount reacted.
  • N A K L a (C o - C1) (l3)
  • K L a mass transfer coefficient
  • the rating of the system is based on the total air flow to nozzle 30.
  • the oxygen transfer rate, OTR in millimols per liter-hour equals 309.
  • nozzle 30 can accept twice this air flow and nozzles 50, 52 will still have capacity to transfer all oxygen back into the liquid. Therefore, the range of operation for the above example is 309-620 millimols per liter-hour.
EP87105515A 1986-04-14 1987-04-14 Gas-Flüssigreaktor und Verfahren zum Mischen von Gas mit Flüssigkeit Expired - Lifetime EP0242776B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US851725 1986-04-14
US06/851,725 US4683122A (en) 1986-04-14 1986-04-14 Gas-liquid reactor and method for gas-liquid mixing

Publications (2)

Publication Number Publication Date
EP0242776A1 true EP0242776A1 (de) 1987-10-28
EP0242776B1 EP0242776B1 (de) 1990-02-07

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EP87105515A Expired - Lifetime EP0242776B1 (de) 1986-04-14 1987-04-14 Gas-Flüssigreaktor und Verfahren zum Mischen von Gas mit Flüssigkeit

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US (1) US4683122A (de)
EP (1) EP0242776B1 (de)
DE (1) DE3761612D1 (de)

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EP0580403A1 (de) * 1992-07-24 1994-01-26 Texaco Chemical Inc. Reaktion von Sauerstoff mit Isobutan nach der Thermosyphon-Methode
EP0679433A1 (de) * 1994-04-25 1995-11-02 Praxair Technology, Inc. Verfahren und Vorrichtung zum Mischen eines kalten Gases mit einer heissen Flüssigkeit
CN102350295A (zh) * 2011-08-06 2012-02-15 河南兴发精细化工有限公司 葡萄糖酸生产中所用空气的预处理方法

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CN104028178B (zh) * 2013-03-06 2016-03-02 中石化上海工程有限公司 强化水力学反应器混合效果的方法
TWI788364B (zh) 2017-06-23 2023-01-01 美商陶氏科技投資有限公司 氫甲醯化反應製程
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US4683122A (en) 1987-07-28
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